An anion double-walled metal-organic framework [CoLi(BTC)(DMF)(HO)·(CH)N] () based on heterobimetallic Li and Co ions was successfully constructed. Utilizing selective destruction and formation of Co-O/Co-N bonds in the metal chains, [CoLi(BTC)(py)(HO)·(CH)N] () and [CoLi(BTC)(pi)(HO)·(CH)N] () with the same skeleton but distinct pore structures can be surprisingly obtained. Additionally, compounds and can be transformed into [CoLi(BTC)(HO)·(CH)N] () by soaking them in an ethanol solution. This kind of single-crystal-to-single-crystal transformation successfully regulates the pore structure of MOFs and enriches the diversity of the pore wall on the premise of retaining the original framework. Most impressively, compound shows high adsorption capacity for Cs cations and is a good candidate to selectively accommodate Cs among the common alkali metal ions, which is future identified by single-crystal X-ray diffraction and inductively coupled plasma mass spectrometry (ICP-MS) test. Meanwhile, compound can selectively adsorb methylene blue (MB) and crystal violet (CV) molecules over Rhodamine B (RMB).
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